Revealing the roles of the solid–electrolyte interphase in designing stable, fast-charging, low-temperature Li-ion batteries

Designing the solid-electrolyte interphase (SEI) is critical for stable, fast-charging, low-temperature Li-ion batteries. Fostering a "fluorinated interphase," SEI enriched with LiF, has become a popular design strategy. Although LiF possesses low Li-ion conductivity, many studies have reported favorable battery performance with fluorinated SEIs. Such a contradiction suggests that optimizing SEI must extend beyond chemical composition design to consider spatial distributions of different chemical species. In this work, we demonstrate that the impact of a fluorinated SEI on battery performance should be evaluated on a case-by-case basis. Sufficiently passivating the anode surface without impeding Li-ion transport is key. We reveal that a fluorinated SEI containing excessive and dense LiF severely impedes Li-ion transport. In contrast, a fluorinated SEI with well-dispersed LiF (i.e., small LiF aggregates well mixed with other SEI components) is advantageous, presumably due to the enhanced Li-ion transport across heterointerfaces between LiF and other SEI components. An electrolyte, 1 M LiPF<sub>6</sub> in 2-methyl tetrahydrofuran (2MeTHF), yields a fluorinated SEI with dispersed LiF. This electrolyte allows anodes of graphite, μSi/graphite composite, and pure Si to all deliver a stable Coulombic efficiency of 99.9% and excellent rate capability at low temperatures. Pouch cells containing layered cathodes also demonstrate impressive cycling stability over 1,000 cycles and exceptional rate capability down to -20 °C. Through experiments and theoretical modeling, we have identified a balanced SEI-based approach that achieves stable, fast-charging, low-temperature Li-ion batteries.

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Publication Details

Journal
Proceedings of the National Academy of Sciences
Published
2025-03-24
DOI
https://doi.org/10.1073/pnas.2420398122
Citations
9
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
6.57

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article

Revealing the roles of the solid–electrolyte interphase in designing stable, fast-charging, low-temperature Li-ion batteries

Joshua Russell, Zhaohui Liang, Chenguang Shi, J. C. K. Lai et al.
9 citations
Proceedings of the National Academy of Sciences
Advancements in Battery Materials
6.57
article

Revealing the roles of the solid–electrolyte interphase in designing stable, fast-charging, low-temperature Li-ion batteries

Joshua Russell, Zhaohui Liang, Chenguang Shi, J. C. K. Lai, Hui Xiong, Louis A. Madsen, Feifei Shi, Kejie Zhao, Sameep Rajubhai Shah, Sooyeon Hwang, Deyang Yu, Feng Lin, Weibo Huang, Dawei Xia, Lei Tao, Yanjun Guo, Hanrui Zhang, Jungki Min, Xixian Yang
article en
9 citations

Abstract

Designing the solid-electrolyte interphase (SEI) is critical for stable, fast-charging, low-temperature Li-ion batteries. Fostering a "fluorinated interphase," SEI enriched with LiF, has become a popular design strategy. Although LiF possesses low Li-ion conductivity, many studies have reported favorable battery performance with fluorinated SEIs. Such a contradiction suggests that optimizing SEI must extend beyond chemical composition design to consider spatial distributions of different chemical species. In this work, we demonstrate that the impact of a fluorinated SEI on battery performance should be evaluated on a case-by-case basis. Sufficiently passivating the anode surface without impeding Li-ion transport is key. We reveal that a fluorinated SEI containing excessive and dense LiF severely impedes Li-ion transport. In contrast, a fluorinated SEI with well-dispersed LiF (i.e., small LiF aggregates well mixed with other SEI components) is advantageous, presumably due to the enhanced Li-ion transport across heterointerfaces between LiF and other SEI components. An electrolyte, 1 M LiPF<sub>6</sub> in 2-methyl tetrahydrofuran (2MeTHF), yields a fluorinated SEI with dispersed LiF. This electrolyte allows anodes of graphite, μSi/graphite composite, and pure Si to all deliver a stable Coulombic efficiency of 99.9% and excellent rate capability at low temperatures. Pouch cells containing layered cathodes also demonstrate impressive cycling stability over 1,000 cycles and exceptional rate capability down to -20 °C. Through experiments and theoretical modeling, we have identified a balanced SEI-based approach that achieves stable, fast-charging, low-temperature Li-ion batteries.

Proceedings of the National Academy of SciencesVol. 122(13)
Micron (United States) (US), Boise State University (US), Pennsylvania State University (US), Brookhaven National Laboratory (US), Purdue University West Lafayette (US), Mineral Resources (AU), Virginia Tech (US)
National Science Foundation, U.S. Department of Energy, Advanced Research Projects Agency - Energy, Office of Science, Advanced Research Projects Agency, Division of Materials Research, Division of Chemical, Bioengineering, Environmental, and Transport Systems, Division of Civil, Mechanical and Manufacturing Innovation, Brookhaven National Laboratory
Openalex Percentile: Top 3%
Advancements in Battery Materials
6.57
DOIOpen Access PDFOpenAlex
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